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09/13/07 - USPTO Class 525 |  94 views | #20070213473 | Prev - Next | About this Page  525 rss/xml feed  monitor keywords

Composition and method of use

USPTO Application #: 20070213473
Title: Composition and method of use
Abstract: A method for improving at least one property of a polyester, the property selected from the group consisting of impact strength, color, or tensile modulus of a polyester comprising reacting the polyester with an epoxy silane wherein the epoxy is attached to a terminal cycloaliphatic ring system, the reaction product having improved at least one of the properties of impact strength, color, and tensile modulus. (end of abstract)



Agent: Geam - O8cv - CppIPLegal - Pittsfield, MA, US
Inventors: Claire Qing Yu, Dominique Arnould, Kenneth Frederick Miller, Sung Dug Kim, Ning Lu
USPTO Applicaton #: 20070213473 - Class: 525446000 (USPTO)

Related Patent Categories: Synthetic Resins Or Natural Rubbers -- Part Of The Class 520 Series, Natural Rubber Compositions Having Nonreactive Materials (dnrm) Other Than: Carbon, Silicon Dioxide, Glass Titanium Dioxide, Water, Hydrocarbon, Halohydrocarbon, Ethylenically Unsaturated Reactant Admixed With A Preformed Reaction Product Derived From: (a) At Least One Polycarboxylic Acid, Ester, Or Anhydride; (b) At Least One Polyhydroxy Compound; And (c) At Least One Fatty Acid Glycerol Ester, Or A Fatty Acid Or Salt Derived From A Naturally Occurring Glyceride, Tall Oil, Or A Tall Oil Fatty Acid, Solid Polymer Derived From At Least One Carboxylic Acid Or Derivative, Solid Polymer Derived From At Least One Lactam; From An Amino Carboxylic Acid Or Derivative; Or From A Polycarboxylic Acid Or Derivative, Solid Polymer Derived From Polyhydroxy Reactant And Polycarboxylic Acid Or Derivative Reactant; Or Derived From Di- Or Higher Ester Of A Polycarboxylic Acid As Sole Reactant, Mixed With Silicon-containing Reactant Or Polymer Derived Therefrom

Composition and method of use description/claims


The Patent Description & Claims data below is from USPTO Patent Application 20070213473, Composition and method of use.

Brief Patent Description - Full Patent Description - Patent Application Claims
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BACKGROUND OF THE INVENTION

[0001] Polyesters are well known in polymer chemistry for many decades. Among the properties for which polyesters are known are electrical, HDT, flow rate, solvent resistance, and the like. When used in blends with the materials such as polycarbonates, impact modifiers and the like, it is usually the above-mentioned polyester properties which are sought after.

[0002] We have now found that a polyester's [polybutylene terephthalate (PBT)] basic properties of impact strength, color, and tensile modulus can be significantly improved when the polyester is contacted with an epoxysilane, wherein the epoxy is attached to a terminal cycloaliphatic ring system. When the epoxy is attached to a normal alkylene group, no significant improvement in these properties is observed.

SUMMARY OF THE INVENTION

[0003] In accordance with the invention there is a method for improving at least one of the properties of impact strength, color, and tensile modulus of a polyester comprising reacting the polyester with an epoxy silane wherein the epoxy is attached to a terminal cycloaliphatic ring system, the reaction product having improved at least one of the properties of impact strength, color, and tensile modulus.

[0004] Additionally, there is a composition comprising a polyester reacted with an epoxysilane, the product of said reaction having improved at least one of the properties of impact strength, color, and tensile modulus compared to the initial polyester.

DETAILED DESCRIPTION OF THE INVENTION

[0005] The singular forms "a", "an", and "the" include plural referents unless the context clearly dictates otherwise.

[0006] "Optional" or "optionally" as used herein means that the subsequently described event may or may not occur, and that the description includes instances where the event occurs and the instances where it does not occur.

[0007] Any polyester can be the initial polyester provided it has carboxyl and/or alcohol end groups available for reaction with the epoxy silane. Such polyesters include those comprising structural units of formula 1: wherein each R.sup.1 is independently a divalent aliphatic, alicyclic or aromatic hydrocarbon or polyoxyalkylene radical, or mixtures thereof and each A.sup.1 is independently a divalent aliphatic, alicyclic or aromatic radical, or mixtures thereof. Examples of suitable polyesters containing the structure of the above formula are poly(alkylene dicarboxylates), liquid crystalline polyesters, and polyester copolymers. It is also possible to use a branched polyester in which a branching agent, for example, a glycol having three or more hydroxyl groups or a trifunctional or multifunctional carboxylic acid has been incorporated. Furthermore, it is sometimes desirable to have various concentrations of acid and hydroxyl end groups on the polyester, depending on the ultimate end-use of the composition.

[0008] The R.sup.1 radical may be, for example, a C.sub.2-10 alkylene radical, a C.sub.6-12 alicyclic radical, a C.sub.6-20 aromatic radical or a polyoxyalkylene radical in which the alkylene groups contain about 2-6 and most often 2 or 4 carbon atoms. The A.sup.1 radical in the above formula is most often p- or m-phenylene, a cycloaliphatic or a mixture thereof. This class of polyesters includes the poly(alkylene terephthalates). Such polyesters are known in the art as illustrated by the following patents, which are incorporated herein by reference.

[0009] U.S. Pat. Nos. 2,465,319 2,720,502 2,727,881 2,822,348 3,047,539 3,671,487 3,953,394 4,128,526

[0010] Examples of aromatic dicarboxylic acids represented by the dicarboxylated residue A.sup.1 are isophthalic or terephthalic acid, 1,2-di(p-carboxyphenyl)ethane, 4,4'-dicarboxydiphenyl ether, 4,4' bisbenzoic acid and mixtures thereof. Acids containing fused rings can also be present, such as in 1,4-1,5- or 2,6-naphthalenedicarboxylic acids. The preferred dicarboxylic acids are terephthalic acid, isophthalic acid, naphthalene dicarboxylic acid, cyclohexane dicarboxylic acid or mixtures thereof.

[0011] The most preferred polyesters are poly(ethylene terephthalate) ("PET"), poly(1,4-butylene terephthalate) ("PBT"), poly(ethylene naphthanoate) ("PEN"), poly(butylene naphthanoate) ("PBN"), (polypropylene terephthalate) ("PPT"), poly(1,4-10 cyclohexylenedimethylene 1,4-cyclohexanedicarboxylate) ("PCCD"), poly(1,4-cyclohexylenedimethylene terephthalate) ("PCT"), poly(cyclohexylenedimethylene-co-ethylene terephthalate) ("PCTG"), and mixtures thereof.

[0012] Also contemplated herein are the above polyesters with minor amounts, e.g., from about 0.5 to about 5 percent by weight, of units derived from aliphatic acid and/or aliphatic polyols to form copolyesters. The aliphatic polyols include glycols, such as poly(ethylene glycol) or poly(butylene glycol). Such polyesters can be made following the teachings of, for example, U.S. Pat. Nos. 2,465,319 and 3,047,539.

[0013] The epoxy silane which is contacted with and reacts with the polyester is generally any kind of epoxy silane wherein the epoxy is at one end of the molecule and attached to a cycloaliphatic group and the silane is at the other end of the molecule. A desired epoxy silane within that general description is of formula 2. wherein m is an integer 1, 2 or 3, n is an integer of 1 through 6 and X, Y, and Z are the same or different, preferably the same and are alkyl of one to twenty carbon atoms, inclusive, cycloalkyl of four to ten carbon atoms, inclusive, alkylene phenyl wherein alkylene is one to ten carbon atoms, inclusive, and phenylene alkyl wherein alkyl is one to six carbon atoms, inclusive.

[0014] Desirable epoxy silanes within the range are compounds wherein m is 2, n is 1 or 2, desirably 2, and X, Y, and Z are the same and are alkyl of 1, 2, or 3 carbon atoms inclusive. Epoxy silanes within the range which in particular can be used are those wherein m is 2, n is 2, and X, Y, and Z are the same and are methyl or ethyl.

[0015] The polyester modified with the epoxy silane can be blended with any of the usual additives and property modifier that polyesters are usually mixed for example glass, clay, mica and the like. Polymer blends can be made with reacted polyester or can be made with the unreacted polyester and the polyester then reacted with the epoxy silane during the blending or extrusion process. Examples of polymer which can be blended include aromatic polycarbonates, polysulfones, polyethesulfones, impact modifiers, and the like.

[0016] The epoxy silane is reacted with the polyester by simply bringing the two components together at a temperature and time period. For example, PBT 195, Intrinsic Viscosity (IV) 1.1 from GE together with PBT 315, IV 0.7 from GE are tumble blended with various additives such as potassium diphenylsulfone sulfonate (KSS), a flame retardant, a hindered phenol such as Irganox 1010 from Ciba Geigy, a catalyst such as sodium stearate, a mold release such as pentaerythritol tetrastearate (PETS) and the epoxy silane beta-(3,4-epoxycyclohexyl)ethyl triethoxysilane Coatosil 1770 from GE and then extruded in a 27 mm twin screw with a vacuum vented mixing screw at a barrel and die head temperature between 240 and 265 degrees Celsius and 450 ppm screw speed. The extrudate is cooled through a water bath prior to palletizing.

[0017] The quantities of epoxy silane employed as a percentage of polyester present in the composition is generally at least about 0.1 wt % and a minimum of about 0.4 wt % can also be employed. Generally, further increases in desirable properties are not observable beyond a maximum of about 5.0 wt %, but further quantities can be used if desired.

[0018] Various processes can be used to bring about a desired final product. Injection molding, blow molding, compression molding, resin transfer molding, and the like are processes which can be employed.

[0019] As noted previously various properties can be improved such as impact strength, color, and tensile modulus through the use of the epoxy silane. Virtually any part for an application can benefit from one or a combination of at least two of these properties. For instance, in one embodiment, with respect to the impact strength, a reaction product has an improved impact strength that is at least 10%, as compared to a reaction product that does not contain the epoxy silane, measured with Notched IZOD or DYNATUP impact testing techniques. In another embodiment, the improved impact strength can range from 10 to 30%, or more, as compared to a reaction product that does not contain the epoxy silane, measured with Notched IZOD or DYNATUP impact testing techniques. With respect to improved color properties imparted by the epoxy silane to an opaque reaction product, an opaque reaction product of the invention can have a reduced Yellowness Index by Reflectance (YIR) of at least two units, as compared to a reaction product that does not contain the epoxy silane. In another embodiment, an opaque reaction product of the invention can have a reduced Yellowness Index by Reflectance (YIR) from two to eleven units, or more, as compared to a reaction product that does not contain the epoxy silane. With respect to improved color properties imparted by the epoxy silane to a transparent reaction product, a transparent reaction product of the invention can have a reduced Yellowness Index (YI) of at least one unit, as compared to a reaction product that does not contain the epoxy silane. In another embodiment, a transparent reaction product of the invention can have a reduced Yellowness Index (YI) from one to eleven units, or more, as compared to a reaction product that does not contain the epoxy silane. With respect to tensile modulus, a reaction product has an improved tensile modulus that is at least 5%, as compared to a reaction product that does not contain the epoxy silane, measured with tensile testing techniques. In another embodiment, the improved tensile strength can range from 5 to 10%, or more, as compared to a reaction product that does not contain the epoxy silane, measured with tensile testing techniques.

[0020] Below are examples of the invention. These examples relative to their control comparisons show significant improvement in the above-identified areas. Additionally tensile elongation at break in the non-glass filled PBT and tensile elongation at yield in the glass filled PBT shows improvements. These improvements are indeed selective as noted by other tests providing virtually no improvement or potentially some small declines in tested values.

[0021] Tensile properties were tested according to ASTM D648 using Type 1 tensile bars at room temperatures with a crosshead speed of 2 in/min.

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